Process for extracting mucinous substance from plants



- is obtained.

Patented Aug. 13, 1935 PATENT OFFICE PROCESS FOR EXTRACTING MUCINOUSSUBSTANCE FROM PLANTS Harold B. Near and Au 1 and Raymond W.

gust J. Pacini, Evanston, Crosley, Max M. Gerth,

Frank T. Breidlgam, and John D. Kelly, Chicage, 11]., assignors toLibby, McNeil! & Libby, Chicago, 11]., a corporation of Maine NoDrawing. Application April 5, 1933,

Serial No. 664,665

1 Claim.

This invention relates to a process of obtaining a mucilaginous ormucinous vegetable substance by extraction from the seeds, stalks orother parts of the plant from which the substance This invention may beconsidered in conjunction with the applicants co-pending' application,Serial Number 664,664, filed April 5, 1933, wherein a new and improvedcomposition of matter containing as an essential ingredient, extracts ofthis character, is disclosed and claimed.

Said co-pending application recites by,iway of example the mucilaginousor mucinous 1 extract from plants of the Plantago family or other plantswhich are known to contain a similar type of mucilaginous or mucinoussubstance. As a specific example of a member of the Plantago family, maybe. mentioned seeds of the plants Plantago psyllium, Plantago ovate,Plantago major or Plantago lanseola Also plants of the Salvia family maybe mentioned as follows: Salvia chia, S. polystachia, S. patens, S.verbenacea L., S. horminum L., S.- viridls L., etc. The seeds of variousother plants may be used such as those including flax (Linumusitatissimus L.) and quince- (Pyrus cydonia) and related types ofseeds.

Said co-pending application further mentions the mucinous substancesextracted from okra (Hibiscus esculantus) and related plants; Altheaofiicinalis L. and other Malvaceae and any other plants yielding avegetable mucilage or mucinous substance of this general character.

It is mentioned that substances of this origin may be extracted andprepared for the production of new and useful compositions oi matterpossessing properties rendering themserviceable for various commercialpurposes of which may be mentioned, substitutes for animal gelatin, nowvariously employed in the industries.

Said invention also involves the mucilaginous or mucinous extract incombination with suitable shortening agents of which agar-agar may berecited as a specific example for use incertain applications where it ismore desirable to eliminate the long and glairy properties thereof.

Accordingly, the products'of said invention may be produced of anydesired physical form or consistency, including solids, such as powdersor cakes of various sorts; liquids such as solutions or dilutedispersions, or gels, such as jellies or dispersions similar to thoseproduced with the use of animal gelatin. It is contemplated that thecomposition of matter of this invention be applied commercially in anydesired manner for the production of all types of materials for whichanimal gelatin or animal or vegetable mucins have been heretoforeemployed. As a specific application thereof, may be mentioned theproduction of foods or other substances adapted to 10 be takeninternally. 4

It is an object of said invention to utilize the mucilaginous ormucinousextractof vegetable origin for 'the production of the varioussubstances. in commerce such as foods and similar 15 substances forwhich an animal gelatin has been used heretofore.

In connection with the use of this material in substances adapted forinternal consumption, it possesses the special advantages of beingnondigestible and non-assimilable so that it passes through theintestinal tract in its original unaltered condition. This propertygives the material a physiological value which has been recognized bythe medical profession, as illustrated by the fact that psyllium seedsare in certain instances, recommended as a laxative.

It is well known that psyllium seeds possess the property of absorbinglarge quantities of water, swelling, and exuding a mucilaginous ormucinous substance having the physical properties of a clear, glairy,sticky jelly. It is further known that this substance, when present inthe intestinal tract, provides bulk and acts to stimulate peristalsisand further serves as a non-absorbable lubricant which preventsirritation and promotes the free passage of fecal matter. Thisphysiological value is not possessed by animal gelatin.

Furthermore, in considering the vegetable mucilage or mucin herereferred to, it is found that in a jelly form produced in the presenceof moisture, it possesses the physical properties of animal mucin, whichis known to have soothing 45 and healing action upon the lining of thestomach. Accordingly, it is contemplated that this property of thevegetable mucin of this invention may be utilized in the production ofcommercial products serving as substitutes for animal and vegetablemucin as now supplied on the market.

Various methods may be employed for extracting the desired vegetablemucilage or mucinous substance from the particular plant or seedsselected as a suitable source of material sought.

, However, in most instances, the gel or mucin produced in the'processof extraction is viscous, long and glairy, so that it is extremelydiflicult to separate the seed residue from the mucilaginous or mucinousjelly.

Accordingly, this invention relates to a process by which the separationis effected by initially adding a relatively large quantity of watersuch as for instance, approximately ninety-nine parts to one part of thesolid matter constituting the jelly so that the jelly formed is oflimited viscosity and will possess such liquidity as-to enable thesettling of substantially all of the seeds and seed hulls to the bottomof the mass whereby the separation thereof is facilitated by removingthe gel from the top. By way of example, seeds, such as psyllium seeds,are found to yield approximately 20% of their weight in solid matterentering into the gel and therefore the quantity of water will beapproximately 99% or more to 1% of the jelling constituent of the,seeds. The seeds are previously washed with cold water to remove anydirt,,dust and chafl which may be found thereon and thereafter placed inthe desired quantity of water and brought to a boil. Care should betaken at this point to thoroughly stir the seeds to effect theirthorough separation to prevent lumping thereof while the water is stillcold and before any substantial quantity of mucilage has hadanopportunity to exude therefrom. With the seeds thoroughly separatedand disseminated throughout, the cold water may then be heated by anysuitable means such as for instance, steam introduced into a jacketaround the kettle, and brought to a boil which is maintained forapproximately thirty to thirty-five minutes. I'his treatment isproductive of a quantity of clear, transparent, glairy jelly which issufiiciently low in viscosity to permit the settling of the seeds to thebottom by gravity. Separation may then be effected by removing the topjelly layer from the seeds and placing the same on a screen which ispreferably equipped with vacuum mechanism so as to assist in the pullingof the jelly mass through the screen. The screen must be suiiicientlysmall to prevent the passage of the hulls and remaining psyllium seedswhich are relatively small. Thereafter, the jelly-like product obtainedmay be dried in any suitable type of dryer, such as heated pans, for theremoval of all water, whereupon a clear, horny residue results. Thismaterial may then be utilized for any desired use including those nowemploying animal gelatin, it being understood that it may be furtherprocessed in any desired manner so as to produce any desired type offinished product. That is to say, the resultin solid may be ground to arelatively fine powder so that it may be again taken up in the form of ajelly or it may be sold with a large quantity of liquid, such as wateror other solvent or in the form of a gel or dispersion.

It is also understood that the vegetable muscllsginous or mucinoussubstance may be mixed with other substances as hereinafter pointed out.For instance, it may have certain materials incorporated therewithduring its extraction treatment whereby, as a resulting product, itcontains certain other substances, such as a suitable shortening agent.

The invention therefore contemplates that the solid material prepared asabove outlined may be ground to a suitable fineness, which grinding ispreferably accomplished by the use of a swing hammer grinding mechanismwhich is found to perform this function with a high degree of success.Further, the degree of subdivision is important if it is desiredconveniently, again to convert the powder so .produced, into a jelly, bythe absorption of water. If the material is relatively coarse, asolution with water is formed relatively slowly, butwhen subdivided tothe size of a hundred mesh or smaller, solutions can be obtained withina commercially practical period of time.

As a specific aspect of this invention, it may be mentioned that powderof the above described type is improved by incorporating with it arelatively large quantity of some suitable substance, such as sugar,which acts in the presence of the moisture to separate the individualparticles of the mucilaginous or mucinous product thereby to preventlumping of the same. Sugar may be added to various products adapted forinternal consumption all in accordance with the specific formulahereinafter given, but in other uses, it is contemplated that sugarcrystals may be moistened and thereafter each crystal coated with therelatively fine particles of mucilaginous or mucinous material.Furthermore, the powdered material may be mixed with the desiredquantity of powdered sugar and prepared as a finished powdered productor if desired, pressed into cakes of any desired size and shapewhich maybe, for instance, in the form of pills, adapted for internalconsumption.

Where it is desired to prepare products, the character of which requiresan elimination of the long, sticky, glairy character of the vegetablemucilage or mucin, such as for instance, when jellies are formed, or areintended to be formed from the powder sold in commerce, it is preferableto utilize in conjunction with the vegetable mucilage, a suitableshortening agent, so that if a jelly is prepared to be used as asubstitute for animal jelly in the preparation of desserts or the like,the jelly can be readily cut with a spoon with the elimination of therelatively glairy, sticky properties which are inherent in certain ofthe natural mucilaginous or mucinous substances.

Various shortening agents may be utilized, depending upon the characterof the product to be 'made, but agar-agar may be here recited as onewhich is suitable for the preparation of jellies suitable for internalconsumption.

The following substances may be substituted in whole or in part foragar-agar as shortening agents 1. e. to alter or disguise the mucinous,glairy character of the material and make it more palatable, to cut downropiness, to produce hardness, rigidity, brittleness, etc.

1. Products form alga and other marine plants.

A. Extract from Irish moss (chondrus crispus) and related plants.

B. Extract prepared by the use of alkaline solvents irom Gellidum comeumand related plants.

C. Extract prepared by the use of neutral or alkaline solvents fromvarious species of Lamin::ri)a and related plants (L. agardhii, L.japomica, e

D. Extract prepared by the use of neutral or alkaline solvents fromvarious species of Macrocystis (M. pyrifera, etc.)

E. Extract from various species of Fucus (F. serratus, etc.).

II. Products from land plants.

A. Gum arabic B. Dextrin C. Karaya or Indian gum D. Starch E. TragacanthF. Pect'in and pectinous substances G. Extract of salep and relatedOrchidacea'e III. Animal products.

A. Gelatin B. Isinglass IV. Synthetic products.

A. dibenzoyl l. cystine It is to be understood that this inventioncontemplates other shortening agents such as would be known to bestowthe desired shortening properties upon the particular vegetable mucilageor mucin employed. Of course the shortening agent selected must besuitable for the use intended and in addition, must impart theproperties of friability, brittleness and rigidity to the vegetablesubstance.

In the production of a food product, such as a powder adapted to be usedin the formation of jellies, for the production of desserts and thelike, or liquids for drinks agar-agar can be used satisfactorily as theshortening agent. In such case, the agar may be added to the product byany one of several methods, such as for instance, adding the solidmaterial to the water in which the seeds are originally soaked andboiled. As previously mentioned, approximately ninety-nine parts ofwater are preferably used to one part of solid material constituting thegel, which quantity of water is sumcient to dissolve the required amountof agar-agar.

By way. of example, agar is preferably used in quantity of three andone-half parts to every four and one-half parts of the solid matterconstituting the gel. When the extraction of the vegetable jelly fromthe seeds is completed, that is, after'the cooking process has been runfor the requisite period of time, the agar-agar is thoroughly dissolved,wherefore after the separation process, the resulting jelly contains thepreferred amount of agar as a shortening ingredient. The shorteningagent may be taken into solution and added to the muclnous dispersionbefore or after separation of the seeds or other material of the plantto be separated therefrom.

Where a powdered product is produced from which gels or dispersions areto be subsequently formed, it is desirable that the product be slightlyacid in character for the production of the best results. Care must betaken to avoid the presence of a pH lower than approximately 2, becausea more acid condition acts to destroy to some extent, the jellingproperties. In those cases where the gel is to be used for a food, suchas a substitute for animal gelatin in the production of Jelly dessertsand salads or the like, it is preferable to avoid a pH greater thanapproximately 5 because in certain instances, such as for instance, whenthe mucilaginous or muclnous extract from psyllium seed is employed, ahigher pH is found to result in an undesirable color. In the productionof products where the color is unimportant, the pH may be as high as 8or 9, without danger of securing an undesirable product.

In the production of jellies for use as food products, such as saladsand desserts, the relatively weak acid condition is convenientlyproduced by the presence of certain acid which may be added as anincident to the production of the desired flavor for the food product.For instance, in many such compounds, flavorings of the various fruitsor other substances where the presence of "an acid is important in theproduction of the desired flavor are used and in connection with the useof such flavorings, this invention contemplates the addition of therequisite amount of acid, such as citric, tartaric, malic or any othersimilar acids satisfactory for the production of the desired sour taste.

In the production of jellies for use in making salads and desserts, andlike. food products in which the desired flavoring requires a quantityof acid such as would produce an unfavorable pH, namely, a pH of belowapproximately 2, a

a smaller amount of acid may be used in quantity suflicient to maintainthe hydrogen ion concentration within desired range, together withcertain buffering agents which will act at the time the jelly is takenin the-mouth to maintain the desired acidity with the consequentmaintenance of taste. As suitable buffering agents, may be mentionedsodium or potassium citrate, or sodium and potassium di or mono hydrogenphosphate, glycocoll, or any other known and suitable buffering agents.

A typical example for the production of a powdered product from whichfood jellies may be made such as desserts, salads and the like, is asfollows:

Psyllium mucilaginous or muclnous extract 4. 44 4. 5 Agar-agar 3. 56 3.6 Tartanc acid 2. 50 2. 5 Sodium citrate. 1. 00 l. 0 Sugar L 87.00 88.4

ance with the above description and the other ingredients added theretoafter the powder has been formed. If it is desired, the otheringredients, such as sugar, the acid, and buffer, etc., may be groundwith the mucinous and shortening substances. The powder so prepared canthenbe sold on the market for the dual purpose of serving as a foodmaterial and as a pleasant form of dosage for the requisite quantity ofmuclnous compound with its desired physiological value.

The jelly formed from the powder so prepared is produced by adding therelatively large quantity of water approximately five times the volumeof the powder employed, and thereby effecting a dispersion of thejelling constituency. If the substance is'added to cold water, a gelwill be formedonly with great difliculty and prolonged standingwherefore it is contemplated that the powders added to cold water orother liquid may serve for the production of appetizing drinks which arenot only tasteful and pleasant to take, but are also rich in the desiredquantity of vegetable mucinous substance which provides a desirablephysiological action. When the powder is taken up in hot water, a gel isformed but firmer gel is produced when the water is boiled.

The hot or boiling water serves to disperse the jelling constituencywhich promptly sets and forms the finished gel in a relatively short pc-'seedssinktothebottomofthe riod of time. Satisfactory gels for thepurpose of desserts, and salads or the like, may be formed in aboutone-third to one-half the time required for the jelling of similarproducts produced from animal gelatin. Furthermore, the gels so producedare not softened to any appreciable extent byexposure to highertemperatures, such as room temperature, after removing from the ice box.

It is to be understood that jellied products are mentioned only as onepossible form of the present invention as it contemplates the productionof shortened or non-shortened compositions for various uses, forinstance, as substitutes for animal mucin as nowgadministered for thetreatment of stomach disorders. Furthermore, the materials may beprepared for the market, as liquids, solids, gels or any other desiredform. As solids, the mucilaginous or mucinous substance may be sold as apowder or in cake form such as for ce, as pills or any other size andshape of cake.

It is to be unders that the material may be either pure or mixed withother ents, all in the er herein specified and recited by way ofexample.

Other specific examples for producing compositions in accordance withthis invention are as follows:

Example 1 Ten pounds of seeds of the Plantago psyllium are thoroughlywashed with cold water. They are then mixed with four hundred pounds ofwater in a steam-jacketed kettle. The contents of the kettle'are broughtto a boil and boiled intermittently for twenty-five minutes more orless. The contents of the kettle are then allowed to rest quietly forten minutes. The extracted kettle leaving a thick liquid above which isrelatively clear of Any debris collected on the top is skimmed oil." Theclear, glairy mass is decanted and filtered through a wire gauze by'theuse of either pressure or vacuum. The filtered mass is placed in shallowpans and dried in a current of warm air. The resulting product consistsof dark colored scales or. plates which are more or less flexible andhorny. The scales are ground to' a powder. The above seeds should yieldabout one pound of dry extract.

One pound of the dried extract is mixed with four-fifths of a pound ofagar-agar and stirred into fifty pounds of cold water. After soaking forone hour the mixture is brought to boiling and boiled for flveminutes'more or less. Upon cooling this mixture sets to a tough,rubbery, moreorlessrigidmsss. Thismassiscutin small pieces and dried ina current of hot air. The dry product possesses ties of animal gelatin.For example, when placed in cold waterit swells. When one part is heatedwith ninety-nine parts of water to a temperature near the boiling pointit apparently dissolves and upon cooling sets to a gel which closelyresembles a gelatin gel.

Example 2 I'ive pounds of the seeds of Plantago ovate are washed withcold water and are placed in a steam-jacketed kettle together with twohundred and ility pounds of water. The mixture is brought to a boil andis boiled intennittently for twenty five minutes more or becomesrelatively clear.

theglsirrllq dabove many of the properless. It is then to stand quietlyfor ten minutes more or It is decanted and filtered through a wirescreen.

Four-fliths of a pound of agar-agar are soaked for one hour in fiftypounds of water, are brought to a boil and boiled until the agar-agarhas become uniformly dispersed in the water. This liquid is added to thehot extract of the Plantago seeds and thoroughly mixed therewith and themixture brought to boiling. Upon cooling, this mixture sets to a gelwhich is similar in physical properties to a rather dilute gelatin gel.This gel may be dried in a current of air or it may be melted and driedby spraying into a heated chamber or it may be dried in a vacuum pan.The resulting product possesses many of the properties of animalgelatin. It swells in cold water and disperses in boiling water to forma solution which sets to a gel upon cooling.

Example 3 Five pounds of the seeds of Plantago ovate are washed in coldwater and are placed in a steamplated kettle together with two hundredand fifty pounds of water. The mixture is brought to a boil and boiledintermittently for twenty flve minutes more or less. The mixture is.allowed to set quietly for ten minutes more or less. The seeds settle tothe bottom leaving a more or less clear liquid above. The clear liquidis decanted and filtered through a wire gauze.

Three-fourths of a pound of agar-agar is soaked in cold water for onehour. The swollen agar is drained, is added to the filtered Plantagoextract and the mixture is boiled until the agaragar is thoroughlydissolved. Upon cooling, this liquid sets to a gel which resembles inphysical properties a gel made from animal gelatin. It may be dried orotherwise treated as desired.

Example 4 Five-sixths of a pound of agar-agar is soaked in two hundredand fifty pounds of waterfor one hour. It is transferred to asteam-jacketed kettle and brought to a boil and boiled until theagar-agar is thoroughly dispersed; Five pounds of the seeds of Plantagoovate are thrown into the boiling liquid and the boiling is continuedintermittently for twenty five minutes more or less. The mass is allowedto rest quietly for ten minutes more or less. The extracted seeds settleto the bottom leaving a clear liquid above. This clear liquid isdecanted and filtered through a wire screen. Upon cooling, it sets to agel which resembles in physical properties a gel made from animalgelatin. It may lee-dried or otherwise treated as desired.

In conclusion, it may be mentioned that the physiological value oi. themucinous. extract utilized in the practice of this invention is based,in part, upon the following considerations:

The demulcent properties of psyllium, cydonium, and like vegetablemucins have been thera peuticaily recognized in the oflicialPharmacopmias, Dispensatories, Codexes, and other formularies of variousnations. The difliculty of providing these demulcent properties to theexclusion of a mechanical irritation produced by the insoluble kernelhas withheld a more popular use of this-product. This inventiondiscloses the method whereby the vegetable mucin properties of psylliumand like vegetable mucins can be obtained to the exclusion of theirritating dbris, thus furnishing an article of pharmaceutical elegancesuitable ior the'treatment of gastro-enteric disorders where not onlylubrication dueto indigestible mucins, demulcent properties", enzyme-.to a biochemist are self evident and are included.

absorbing properties, and addition to fecal bulk, but Where also many ofthe properties of animal mucin are reduplicated and made available.Particularly is it to be noted that those ulcerative conditions of thegastro-intestinal tract, diverticulus conditions, and other lesionswherein demulcents are indicated but psyllium and like seeds have beenstrictly contra-indicatedby reason of the irritating debris factor, nowbecome fully available for treatment through the agency of the vegetablemucins typically represented by this invention. I

It must not be overlooked that the preparation lends itself to use notonly as an improved medicinal agent, but as a dietary article replacingin many instances the pectinous materials, aspics, and the like.Thus,'the gels of various fruits can be fortified by the use of thebland vegetable mucin represented by this invention, and manyadvantageous qualities added thereto.

The modifications of the properties of the vegetable mucins through theco-addition of vegetable galtin, Indian gum and a variety of similarsubstances very readily suggesting themselves in the scope of thisinvention.

We claim:

The process which comprises subjecting vegetable material containingmucilage of the type obtainable from the seeds of Plantago psyllium tothe action of boiling water until the mucilage therein has swelled andis rendered exteriorly of the cellulosic and other portions of saidmaterial, then separating the dispersed mucilage from the cellulosic andother portions of said material by permitting the latter to settle bygravity under conditions of low viscosity by dilution with water having-agar-agar dispersed therein, said agaragar serving to reduce thestickiness of said dispersed mucilage and producing a condition whichpermits said separation more easily and thereafter separating the topclean'layer of mucilage and dispersed agar. HAROLD. B. NEAR. AUGUST J.PACINI. RAYMOND W. CROSLEY. MAX M. GERTH.

FRANK T. BREIDIGAM. JOHN D. KELLY.

